We have fabricated switchable gas permeation membranes in which a photoswitchable low-molecular-weight liquid crystalline (LC) material acts as the active element. Liquid crystal mixtures are doped with mesogenic azo dyes and infused into commercially available track-etched membranes with regular cylindrical pores (0.40 to 10.0 μm). Tunability of mass transfer can be achieved through a combination of (1) LC/mesogenic dye composition, (2) surface-induced alignment, and (3) reversible photoinduced LC-isotropic transitions. Photo-induced isothermal phase changes in the imbibed material afford large and fully reversible changes in the permeability of the membrane to nitrogen. Both the LC and photogenerated isotropic states demonstrate a linear permeability/pressure relationship, but they show significant differences in their permeability coefficients. Liquid crystal compositions can be chosen such that the LC phase is more permeable than the isotropic—or vice versa – and can be further tuned by surface alignment. Permeability switching response times are 5 s, with alternating UV and >420-nm radiation at an intensity of 2 mW/cm2 being sufficient for complete and reversible switching. Thermal and kinetic properties of the confined LC materials are evaluated and correlated with the observed permeation properties. We demonstrate for the first time reversible permeation control of a membrane with light irradiation.